14,216 results on '"exciton"'
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2. Vertical Electric-Field-Induced Switching from Strong to Asymmetric Strong–Weak Confinement in GaAs Cone-Shell Quantum Dots Using Transparent Al-Doped ZnO Gates.
- Author
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Alshaikh, Ahmed, Peng, Jun, Zierold, Robert, Blick, Robert H., and Heyn, Christian
- Subjects
- *
QUANTUM rings , *SEMICONDUCTOR junctions , *INTEGRATED circuits , *SEMICONDUCTOR materials , *AUDITING standards , *QUANTUM dots , *SEMICONDUCTOR quantum dots - Abstract
The first part of this work evaluates Al-doped ZnO (AZO) as an optically transparent top-gate material for studies on semiconductor quantum dots. In comparison with conventional Ti gates, samples with AZO gates demonstrate a more than three times higher intensity in the quantum dot emission under comparable excitation conditions. On the other hand, charges inside a process-induced oxide layer at the interface to the semiconductor cause artifacts at gate voltages above U ≈ 1 V. The second part describes an optical and simulation study of a vertical electric-field (F)-induced switching from a strong to an asymmetric strong–weak confinement in GaAs cone-shell quantum dots (CSQDs), where the charge carrier probability densities are localized on the surface of a cone. These experiments are performed at low U and show no indications of an influence of interface charges. For a large F, the measured radiative lifetimes are substantially shorter compared with simulation results. We attribute this discrepancy to an F-induced transformation of the shape of the hole probability density. In detail, an increasing F pushes the hole into the wing part of a CSQD, where it forms a quantum ring. Accordingly, the confinement of the hole is changed from strong, which is assumed in the simulations, to weak, where the local radius is larger than the bulk exciton Bohr radius. In contrast to the hole, an increasing F pushes the electron into the CSQD tip, where it remains in a strong confinement. This means the radiative lifetime for large F is given by an asymmetric confinement with a strongly confined electron and a hole in a weak confinement. To our knowledge, this asymmetric strong–weak confinement represents a novel kind of quantum mechanical confinement and has not been observed so far. Furthermore, the observed weak confinement for the hole represents a confirmation of the theoretically predicted transformation of the hole probability density from a quantum dot into a quantum ring. For such quantum rings, application as storage for photo-excited charge carriers is predicted, which can be interesting for future quantum photonic integrated circuits. [ABSTRACT FROM AUTHOR]
- Published
- 2024
- Full Text
- View/download PDF
3. Existence of symmetry-broken excited states in single and ensemble quantum ring structures
- Author
-
Jang, Hyoseong, Jeon, Seung Kwon, Jeong, Seungmin, and Kim, Heedae
- Published
- 2024
- Full Text
- View/download PDF
4. Competition between Phonon-Assisted and Exciton Photoluminescence Modulated by Temperature in WSe2/Graphene Nanosheet Heterostructures for Flexible Optoelectronic Sensor Devices.
- Author
-
Ruowei Wu, Chuan He, Xiangxin Meng, Hui Tan, Weiming He, Jianfeng Xu, Debin Ren, Xuzhang Duan, Lipeng Zhu, and Qiyi Zhao
- Abstract
Temperature field engineering provides a robust framework for investigating the behavior of phonons and excitons within two-dimensional (2D) layered van der Waals materials. Herein, we measured the photoluminescence (PL) spectroscopy of few-layer WSe
2 and WSe2 /graphene van der Waals heterostructures at various temperatures (from 10 to 300 K). The results indicate that the PL intensity of the heterostructure is lower than that of few-layer WSe2 , which is attributed to charge transfer at the interface under photoexcitation conditions. The PL spectroscopy spectrum of the heterostructure is primarily composed of four distinct spectral features, arising from distinct phonon-assisted processes, direct recombination, and excitonic contributions. Furthermore, these physical processes can be modulated by varying the temperature. For instance, the phonon-assisted PL process gradually diminishes with the decrease in temperature, whereas the excitonic PL process emerges more distinctly with the reduction in temperature. These findings can provide support for understanding the photophysical processes in 2D heterostructure materials and lay the groundwork for optoelectronic devices based on nanomaterials. [ABSTRACT FROM AUTHOR]- Published
- 2024
- Full Text
- View/download PDF
5. GaAs Cone-Shell Quantum Dots in a Lateral Electric Field: Exciton Stark-Shift, Lifetime, and Fine-Structure Splitting.
- Author
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Alshaikh, Ahmed, Blick, Robert H., and Heyn, Christian
- Subjects
- *
ELECTRIC charge , *ELECTRIC fields , *SURFACE charges , *MAGNETIC fields , *VOLTAGE , *QUANTUM dots - Abstract
Strain-free GaAs cone-shell quantum dots have a unique shape, which allows a wide tunability of the charge-carrier probability densities by external electric and magnetic fields. Here, the influence of a lateral electric field on the optical emission is studied experimentally using simulations. The simulations predict that the electron and hole form a lateral dipole when subjected to a lateral electric field. To evaluate this prediction experimentally, we integrate the dots in a lateral gate geometry and measure the Stark-shift of the exciton energy, the exciton intensity, the radiative lifetime, and the fine-structure splitting (FSS) using single-dot photoluminescence spectroscopy. The respective gate voltage dependencies show nontrivial trends with three pronounced regimes. We assume that the respective dominant processes are charge-carrier deformation at a low gate voltage U, a vertical charge-carrier shift at medium U, and a lateral charge-carrier polarization at high U. The lateral polarization forms a dipole, which can either enhance or compensate the intrinsic FSS induced by the QD shape anisotropy, dependent on the in-plane orientation of the electric field. Furthermore, the data show that the biexciton peak can be suppressed by a lateral gate voltage, and we assume the presence of an additional vertical electric field induced by surface charges. [ABSTRACT FROM AUTHOR]
- Published
- 2024
- Full Text
- View/download PDF
6. Exciton and Trion at the Perimeter and Grain Boundary of CVD-Grown Monolayer MoS2: Strain Effects Influencing Application in Nano-Optoelectronics.
- Author
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Golovynskyi, Sergii, Datsenko, Oleksandr I., Pérez-Jiménez, Ana I., Kuklin, Artem, Chaigneau, Marc, Golovynskyi, Andrii, Golovynska, Iuliia, Bosi, Matteo, and Seravalli, Luca
- Abstract
Nanolayers of MoS
2 can be grown to be used as active elements in nano-optoelectronic devices such as two-dimensional (2D) light emitters and optical detectors. The growth of 2D flakes might result in the formation of not only isolated triangles but also complex polycrystal flakes when different flakes interact during their in-plane expansion. In this paper, we investigate how monolayer MoS2 flakes of different shapes are affected by the biaxial strain resulting from the cooling process after chemical vapor deposition growth. The single- and polycrystal flakes are characterized at the nanoscale level by correlating morphological, electrical, and optical measurements and imaging. The main focus is given to the analysis of the exciton/trion photoluminescence (PL) components extracted from the spectra at different areas of the flake surface. According to the Raman imaging, the whole flake has built-in heterogeneous tensile strain, with the perimeter and the grain boundaries between the single-crystal parts of the poly flakes exhibiting a lower strain level (0.2–0.3%) and the central area being more strained (∼0.4%). At the perimeter and grain boundaries, the PL undergoes the strain-related blueshift accompanied by a weakening of the contribution of the long-wave trion to the spectrum and the trion binding energy. The trion formation is known to be proportional to a local electron concentration. The trion PL imaging compared to the surface potential mapping confirms a decrease in n-doping at the perimeter and grain boundaries, leading to the trion weakening. To confirm the results of electron drift to strained areas of the flake, creating the trion, the band bending at the tensile-strained flake has been theoretically calculated and modeled. The effect of edge defects at the perimeter and grain boundaries on the doping, which leads to the enhancement or inhibition of the trion formation depending on the edge and grain boundary interface type, is also discussed. [ABSTRACT FROM AUTHOR]- Published
- 2024
- Full Text
- View/download PDF
7. Electroluminescence and photocurrent generation in pn-diode of trilayer phosphorene
- Author
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Yoon, Sangho, Kim, Taeho, Song, Su-Beom, Watanabe, Kenji, Taniguchi, Takashi, and Kim, Jonghwan
- Published
- 2024
- Full Text
- View/download PDF
8. Vertical Electric-Field-Induced Switching from Strong to Asymmetric Strong–Weak Confinement in GaAs Cone-Shell Quantum Dots Using Transparent Al-Doped ZnO Gates
- Author
-
Ahmed Alshaikh, Jun Peng, Robert Zierold, Robert H. Blick, and Christian Heyn
- Subjects
Al-doped ZnO ,GaAs quantum dot ,photoluminescence ,exciton ,lifetime ,Stark shift ,Chemistry ,QD1-999 - Abstract
The first part of this work evaluates Al-doped ZnO (AZO) as an optically transparent top-gate material for studies on semiconductor quantum dots. In comparison with conventional Ti gates, samples with AZO gates demonstrate a more than three times higher intensity in the quantum dot emission under comparable excitation conditions. On the other hand, charges inside a process-induced oxide layer at the interface to the semiconductor cause artifacts at gate voltages above U≈ 1 V. The second part describes an optical and simulation study of a vertical electric-field (F)-induced switching from a strong to an asymmetric strong–weak confinement in GaAs cone-shell quantum dots (CSQDs), where the charge carrier probability densities are localized on the surface of a cone. These experiments are performed at low U and show no indications of an influence of interface charges. For a large F, the measured radiative lifetimes are substantially shorter compared with simulation results. We attribute this discrepancy to an F-induced transformation of the shape of the hole probability density. In detail, an increasing F pushes the hole into the wing part of a CSQD, where it forms a quantum ring. Accordingly, the confinement of the hole is changed from strong, which is assumed in the simulations, to weak, where the local radius is larger than the bulk exciton Bohr radius. In contrast to the hole, an increasing F pushes the electron into the CSQD tip, where it remains in a strong confinement. This means the radiative lifetime for large F is given by an asymmetric confinement with a strongly confined electron and a hole in a weak confinement. To our knowledge, this asymmetric strong–weak confinement represents a novel kind of quantum mechanical confinement and has not been observed so far. Furthermore, the observed weak confinement for the hole represents a confirmation of the theoretically predicted transformation of the hole probability density from a quantum dot into a quantum ring. For such quantum rings, application as storage for photo-excited charge carriers is predicted, which can be interesting for future quantum photonic integrated circuits.
- Published
- 2024
- Full Text
- View/download PDF
9. Unveiling the Synergy of Coupled Gold Nanoparticles and J-Aggregates in Plexcitonic Systems for Enhanced Photochemical Applications.
- Author
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Jumbo-Nogales, Alba, Rao, Anish, Olejniczak, Adam, Grzelczak, Marek, and Rakovich, Yury
- Subjects
- *
GOLD nanoparticles , *HYBRID systems , *PHOTOLUMINESCENCE , *EXCITON theory , *PLASMONICS , *MICROSCOPY - Abstract
Plexcitonic systems based on metal nanostructures and molecular J-aggregates offer an excellent opportunity to explore the intriguing interplay between plasmonic excitations and excitons, offering unique insights into light–matter interactions at the nanoscale. Their potential applications in photocatalysis have prompted a growing interest in both their synthesis and the analysis of their properties. However, in order to construct a high-performing system, it is essential to ensure chemical and spectral compatibility between both components. We present the results of a study into a hybrid system, achieved through the coupling of gold nanobipyramids with organic molecules, and demonstrate the strengthened photochemical properties of such a system in comparison with purely J-aggregates. Our analysis includes the absorbance and photoluminescence characterization of the system, revealing the remarkable plexcitonic interaction and pronounced coupling effect. The absorbance spectroscopy of the hybrid systems enabled the investigation of the coupling strength (g). Additionally, the photoluminescence response of the J-aggregates and coupled systems reveals the impact of the coupling regime. Utilizing fluorescence lifetime imaging microscopy, we established how the photoluminescence lifetime components of the J-aggregates are affected within the plexcitonic system. Finally, to assess the photodegradation of J-aggregates and plexcitonic systems, we conducted a comparative analysis. Our findings reveal that plasmon-enhanced interactions lead to improved photostability in hybrid systems. [ABSTRACT FROM AUTHOR]
- Published
- 2024
- Full Text
- View/download PDF
10. Temperature-Enhanced Exciton Emission from GaAs Cone–Shell Quantum Dots.
- Author
-
Heyn, Christian, Ranasinghe, Leonardo, Deneke, Kristian, Alshaikh, Ahmed, and Blick, Robert H.
- Subjects
- *
QUANTUM dots , *MOLECULAR beam epitaxy , *AUDITING standards , *GALLIUM arsenide , *EXCITON theory - Abstract
The temperature-dependent intensities of the exciton (X) and biexciton (XX) peaks from single GaAs cone–shell quantum dots (QDs) are studied with micro photoluminescence (PL) at varied excitation power and QD size. The QDs are fabricated by filling self-assembled nanoholes, which are drilled in an AlGaAs barrier by local droplet etching (LDE) during molecular beam epitaxy (MBE). This method allows the fabrication of strain-free QDs with sizes precisely controlled by the amount of material deposited for hole filling. Starting from the base temperature T = 3.2 K of the cryostat, single-dot PL measurements demonstrate a strong enhancement of the exciton emission up to a factor of five with increasing T. Both the maximum exciton intensity and the temperature T x , m a x of the maximum intensity depend on excitation power and dot size. At an elevated excitation power, T x , m a x becomes larger than 30 K. This allows an operation using an inexpensive and compact Stirling cryocooler. Above T x , m a x , the exciton intensity decreases strongly until it disappears. The experimental data are quantitatively reproduced by a model which considers the competing processes of exciton generation, annihilation, and recombination. Exciton generation in the QDs is achieved by the sum of direct excitation in the dot, plus additional bulk excitons diffusing from the barrier layers into the dot. The thermally driven bulk-exciton diffusion from the barriers causes the temperature enhancement of the exciton emission. Above T x , m a x , the intensity decreases due to exciton annihilation processes. In comparison to the exciton, the biexciton intensity shows only very weak enhancement, which is attributed to more efficient annihilation processes. [ABSTRACT FROM AUTHOR]
- Published
- 2023
- Full Text
- View/download PDF
11. GaAs Cone-Shell Quantum Dots in a Lateral Electric Field: Exciton Stark-Shift, Lifetime, and Fine-Structure Splitting
- Author
-
Ahmed Alshaikh, Robert H. Blick, and Christian Heyn
- Subjects
quantum dot ,photoluminescence ,exciton ,lateral electric field ,exciton energy ,Stark-shift ,Chemistry ,QD1-999 - Abstract
Strain-free GaAs cone-shell quantum dots have a unique shape, which allows a wide tunability of the charge-carrier probability densities by external electric and magnetic fields. Here, the influence of a lateral electric field on the optical emission is studied experimentally using simulations. The simulations predict that the electron and hole form a lateral dipole when subjected to a lateral electric field. To evaluate this prediction experimentally, we integrate the dots in a lateral gate geometry and measure the Stark-shift of the exciton energy, the exciton intensity, the radiative lifetime, and the fine-structure splitting (FSS) using single-dot photoluminescence spectroscopy. The respective gate voltage dependencies show nontrivial trends with three pronounced regimes. We assume that the respective dominant processes are charge-carrier deformation at a low gate voltage U, a vertical charge-carrier shift at medium U, and a lateral charge-carrier polarization at high U. The lateral polarization forms a dipole, which can either enhance or compensate the intrinsic FSS induced by the QD shape anisotropy, dependent on the in-plane orientation of the electric field. Furthermore, the data show that the biexciton peak can be suppressed by a lateral gate voltage, and we assume the presence of an additional vertical electric field induced by surface charges.
- Published
- 2024
- Full Text
- View/download PDF
12. Discrete Donor–Acceptor Pair Transitions in CH3NH3PbI3 Perovskite Single Crystals.
- Author
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Urban, Joanna M., Nguyen, Thi Huyen Trang, Chehade, Gabriel, Delteil, Aymeric, Trippé-Allard, Gaëlle, Delport, Geraud, Deleporte, Emmanuelle, Hermier, Jean-Pierre, and Garrot, Damien
- Subjects
- *
SINGLE crystals , *PEROVSKITE , *CRYSTAL surfaces , *CARRIER density , *PHYSICS , *PHONONS - Abstract
Achieving a better understanding of the physics of defects in halide perovskites (HPs) is a key challenge for improving the efficiency of the devices. Herein, a comprehensive study of the defect emission of CH3NH3PbI3 perovskite single crystals is presented. The emission of the pristine surface of cleaved crystals is systematically investigated based on steady‐state and time‐resolved micro‐photoluminescence (micro‐PL) spectroscopy. Donor–acceptor pair (DAP) recombination is observed due to the presence of native shallow defects. The DAP spectra present an important variability depending on the location on the surface of the crystals due to inhomogeneous defect distribution. A strong blueshift of the emission is measured as a function of excitation power and is explained by fluctuating potential caused by compensated defects. With increasing photocarrier density, a transition from a structureless to a structured DAP emission with several longitudinal optical phonon replicas is observed. The DAP transition is characterized by the redshift of the emission with time and a slow, non‐exponential PL decay. Sharp discrete lines with sub‐meV widths, the most recognizable spectral signature of DAP transition, are revealed. Herein, the apparently contradictory previous observations on defect emission of CH3NH3PbI3 are reconciled by the results and new insights are provided into the properties of defects in HPs. [ABSTRACT FROM AUTHOR]
- Published
- 2023
- Full Text
- View/download PDF
13. Defect Formation of Light-Emitting Particles during the Synthesis of a Hierarchical Porous Surface of ZnO/SiO 2 /Si Structures †.
- Author
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Zhapakov, Rashid, Begunov, Mykhail, Seredavina, Tatyana, Murzalinov, Danatbek, Serikkanov, Abay, Dmitriyeva, Elena, Zhantuarov, Sultan, and Ibraimova, Sayara
- Subjects
SOL-gel processes ,PHOTOLUMINESCENCE ,ZINC oxide ,LIGHT emitting diodes ,HETEROSTRUCTURES - Abstract
The formation of structures of different sizes on the surface of a single sample and the study of the mechanisms of their excitations and energy transitions is a promising area of research. ZnO/SiO
2 /Si heterostructures were formed by two-stage electrochemical etching of silicon wafers and synthesizing zinc oxide nanoparticles using sol-gel technology. By scanning electron and atomic force microscopies, various pores and clusters were identified. The presence of five levels of surface hierarchy provided the synthesis of light-emitting particles with different properties. Light emission mechanisms are associated with the recombination of excitons and the hyperfine structure of charged particles trapped on oxygen vacancy. [ABSTRACT FROM AUTHOR]- Published
- 2023
- Full Text
- View/download PDF
14. Secondary Emission in Bi2Se3
- Author
-
Kung, Hsiang-Hsi and Kung, Hsiang-Hsi
- Published
- 2022
- Full Text
- View/download PDF
15. Optical Properties of Conical Quantum Dot: Exciton-Related Raman Scattering, Interband Absorption and Photoluminescence.
- Author
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Gavalajyan, Sargis P., Mantashian, Grigor A., Kharatyan, Gor Ts., Sarkisyan, Hayk A., Mantashyan, Paytsar A., Baskoutas, Sotirios, and Hayrapetyan, David B.
- Subjects
- *
QUANTUM dots , *RAMAN scattering , *OPTICAL properties , *PHOTOLUMINESCENCE , *EIGENVALUE equations , *LIGHT absorption , *EXCITON theory , *RAMAN effect - Abstract
The current work used the effective mass approximation conjoined with the finite element method to study the exciton states in a conical GaAs quantum dot. In particular, the dependence of the exciton energy on the geometrical parameters of a conical quantum dot has been studied. Once the one-particle eigenvalue equations have been solved, both for electrons and holes, the available information on energies and wave functions is used as input to calculate exciton energy and the effective band gap of the system. The lifetime of an exciton in a conical quantum dot has been estimated and shown to be in the range of nanoseconds. In addition, exciton-related Raman scattering, interband light absorption and photoluminescence in conical GaAs quantum dots have been calculated. It has been shown that with a decrease in the size of the quantum dot, the absorption peak has a blue shift, which is more pronounced for quantum dots of smaller sizes. Furthermore, the interband optical absorption and photoluminescence spectra have been revealed for different sizes of GaAs quantum dot. [ABSTRACT FROM AUTHOR]
- Published
- 2023
- Full Text
- View/download PDF
16. Photoinduced Room-Temperature Magnetism of Low Curie Temperature Cu–Ni Nanoparticles in Polymer Composites with Rubrene Microcrystals.
- Author
-
Rumyantsev, B. M., Bibikov, S. B., Leontiev, V. G., and Berendyaev, V. I.
- Subjects
- *
CURIE temperature , *MAGNETISM , *LOW temperatures , *MAGNETIC nanoparticles , *MAGNETIC moments , *PHOTOTHERMAL effect , *MAGNETIC particles - Abstract
A relation has been established between the decrement of the low-field magnetic spin effect (measured by the luminescence of polymer films of composites with rubrene microcrystals), caused by the addition of magnetic Cu–Ni nanoparticles with a low Curie temperature (TC = 40–60°C), and the photoinduced particle magnetic moment exceeding the dark moment. Based on the study of the temperature dependence of the decrement and its comparison with the thermal demagnetization of the dark magnetic moment, a conclusion was made about a possible mechanism for the photothermal magnetization of nanoparticles. [ABSTRACT FROM AUTHOR]
- Published
- 2023
- Full Text
- View/download PDF
17. Temperature-Enhanced Exciton Emission from GaAs Cone–Shell Quantum Dots
- Author
-
Christian Heyn, Leonardo Ranasinghe, Kristian Deneke, Ahmed Alshaikh, and Robert H. Blick
- Subjects
quantum dot ,photoluminescence ,exciton ,biexciton ,power dependence ,temperature dependence ,Chemistry ,QD1-999 - Abstract
The temperature-dependent intensities of the exciton (X) and biexciton (XX) peaks from single GaAs cone–shell quantum dots (QDs) are studied with micro photoluminescence (PL) at varied excitation power and QD size. The QDs are fabricated by filling self-assembled nanoholes, which are drilled in an AlGaAs barrier by local droplet etching (LDE) during molecular beam epitaxy (MBE). This method allows the fabrication of strain-free QDs with sizes precisely controlled by the amount of material deposited for hole filling. Starting from the base temperature T = 3.2 K of the cryostat, single-dot PL measurements demonstrate a strong enhancement of the exciton emission up to a factor of five with increasing T. Both the maximum exciton intensity and the temperature Tx,max of the maximum intensity depend on excitation power and dot size. At an elevated excitation power, Tx,max becomes larger than 30 K. This allows an operation using an inexpensive and compact Stirling cryocooler. Above Tx,max, the exciton intensity decreases strongly until it disappears. The experimental data are quantitatively reproduced by a model which considers the competing processes of exciton generation, annihilation, and recombination. Exciton generation in the QDs is achieved by the sum of direct excitation in the dot, plus additional bulk excitons diffusing from the barrier layers into the dot. The thermally driven bulk-exciton diffusion from the barriers causes the temperature enhancement of the exciton emission. Above Tx,max, the intensity decreases due to exciton annihilation processes. In comparison to the exciton, the biexciton intensity shows only very weak enhancement, which is attributed to more efficient annihilation processes.
- Published
- 2023
- Full Text
- View/download PDF
18. Mixing of Excitons in Nanostructures Based on a Perylene Dye with CdTe Quantum Dots.
- Author
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Piryatinski, Yuri P., Malynovskyi, Markiian B., Sevryukova, Maryna M., Verbitsky, Anatoli B., Kapush, Olga A., Rozhin, Aleksey G., and Lutsyk, Petro M.
- Subjects
- *
QUANTUM dots , *SEMICONDUCTOR quantum dots , *PERYLENE , *EXCITON theory , *ORGANIC semiconductors , *NANOSTRUCTURES , *DYES & dyeing - Abstract
Semiconductor quantum dots of the A2B6 group and organic semiconductors have been widely studied and applied in optoelectronics. This study aims to combine CdTe quantum dots and perylene-based dye molecules into advanced nanostructure system targeting to improve their functional properties. In such systems, new electronic states, a mixture of Wannier–Mott excitons with charge-transfer excitons, have appeared at the interface of CdTe quantum dots and the perylene dye. The nature of such new states has been analyzed by absorption and photoluminescence spectroscopy with picosecond time resolution. Furthermore, aggregation of perylene dye on the CdTe has been elucidated, and contribution of Förster resonant energy transfer has been observed between aggregated forms of the dye and CdTe quantum dots in the hybrid CdTe-perylene nanostructures. The studied nanostructures have strongly quenched emission of quantum dots enabling potential application of such systems in dissociative sensing. [ABSTRACT FROM AUTHOR]
- Published
- 2023
- Full Text
- View/download PDF
19. On the response of delocalized optoelectronic states in semiconductor coupled quantum dots to remote charge fluctuations
- Author
-
Woodall, Mark Robert
- Subjects
Quantum physics ,Condensed matter physics ,Optics ,Charge Noise ,Exciton ,Optics ,Optoelectronic ,Photoluminescence ,Quantum Dot - Abstract
Solid-state quantum dot molecules (QDMs), systems of two or more coupled quantum dots (QDs), present promising opportunities for creating devices useful for advanced sensing, metrology, communication, and computing operations. In this work, these systems are formed from layered deposition of strained III-V materials that produce spatially aligned nanocrystals capable of charge confinement and susceptible to interdot electron and hole tunneling. When grown in electric field effect structures, the optically generated excitons hosted by these dots are subject to a Quantum Confined Stark Effect (QCSE) which allows for precise and controllable tuning of their energy states and hence their photoluminescence (PL) emissions. These optical transitions are highly sensitive to small fluctuations in the local electronic environment, making them well suited for use in \textit{in situ} nano-scale monitoring. This dissertation reports on the use of QDMs to directly investigate and monitor the physics of interacting quantum states at the single-charge level. In particular, we develop a model that uses intra and interdot excitonic states to precisely characterize the energy splittings induced by remote charges. We make use of low-temperature optical photoluminescence spectroscopy to explore and measure interacting QDM states and document direct interactions between excitonic states and neighboring defect sites and QDMs. We further show how these can be used to locate and monitor remote charges in bulk semiconducting material, with detection ranges $>35\mu$m.Additionally, we develop a model that describes the interactions between neighboring QDM excitonic dipoles, and demonstrate that this interaction gives rise to an engineered state that has reduced sensitivity to remote charge induced fluctuations. Samples with lateral and vertical configurations of QDM molecules are studied, and several promising candidates are identified. This will serve to spur the development of useful quantum devices by allowing for engineering schemes that reduce quantum state sensitivity to charge noise.
- Published
- 2023
20. Dot-Size Dependent Excitons in Droplet-Etched Cone-Shell GaAs Quantum Dots.
- Author
-
Heyn, Christian, Gräfenstein, Andreas, Pirard, Geoffrey, Ranasinghe, Leonardo, Deneke, Kristian, Alshaikh, Ahmed, Bester, Gabriel, and Hansen, Wolfgang
- Subjects
- *
EXCITON theory , *AUDITING standards , *GALLIUM arsenide , *ATOMIC force microscopy , *QUANTUM efficiency , *OSCILLATOR strengths , *QUANTUM dots , *PHOTOLUMINESCENCE measurement - Abstract
Strain-free GaAs quantum dots (QDs) are fabricated by filling droplet-etched nanoholes in AlGaAs. Using a template of nominally identical nanoholes, the QD size is precisely controlled by the thickness of the GaAs filling layer. Atomic force microscopy indicates that the QDs have a cone-shell shape. From single-dot photoluminescence measurements, values of the exciton emission energy (1.58...1.82 eV), the exciton–biexciton splitting (1.8...2.5 meV), the exciton radiative lifetime of bright (0.37...0.58 ns) and dark (3.2...6.7 ns) states, the quantum efficiency (0.89...0.92), and the oscillator strength (11.2...17.1) are determined as a function of the dot size. The experimental data are interpreted by comparison with an atomistic model. [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF
21. Role of H2 in the Substrate-Directed Synthesis of Size-tunable MoSe2 Nanoribbons for Exciton Engineering.
- Author
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Sadler, Erick C., Chowdhury, Tomojit, Dziobek-Garrett, Reynolds, Li, Chenyang, Ambrozaite, Ona, Mueller, Tim, and Kempa, Thomas J.
- Abstract
Recent studies of transition-metal dichalcogenide (TMD) nanoribbons have stimulated the development of synthetic strategies for the controlled growth of these dimensionally restricted crystals. We demonstrate the width-controlled synthesis of MoSe
2 nanoribbons grown on a designer surface comprising Si(001) treated with phosphine. Adjustment of the H2 partial pressure in the carrier gas stream enables the nanoribbon widths to be tuned between 175 nm and almost 500 nm. Experiments and simulations suggest that H2 exposure increases the surface coverage of hydrogen on the Si–P dimers that normally serve as favorable regions for nanoribbon nucleation and growth. Moreover, the MoSe2 nanoribbons exhibit an anomalous photoluminescence blue shift whose magnitude of 60 meV is similar to that reported in optical emission spectra of MoS2 nanoribbons. These studies demonstrate that the recently developed strategy of substrate-directed growth of nanoribbons can be extended to the selenide family of TMDs. Moreover, they expand the synthetic foundation for preparing complex TMD heterostructures, which are required for optical- and quantum-based sensors, transducers, and processors. [ABSTRACT FROM AUTHOR]- Published
- 2022
- Full Text
- View/download PDF
22. Temperature- and Power-Dependent Characteristics of Heterointerlayer Excitons Emitting in the Visible Region of a WS2/PbI2 Nanostructure: Implications in Excitonic Devices.
- Author
-
Kim, Jun Young, Kim, Taek Joon, Lee, Sang-hun, Lee, Eunji, Kim, Jeongyong, and Joo, Jinsoo
- Abstract
Heterointerlayer excitons (HIXs) have been intensively studied in heterostructures of various two-dimensional (2D) nanosystems with staggered band alignment (type II). In this study, the laser confocal microscopy (LCM) photoluminescence (PL) characteristics of exciton species, including HIXs in monolayer (1 L) WS
2 and multilayer PbI2 heterostructures, were investigated from 3 to 293 K. The drastic decrease in the PL intensity of 1 L WS2 after hybridization with multilayer PbI2 indicates the occurrence of charge transfer. PL peaks corresponding to the neutral excitons (X0 ), trions (X– ), and biexcitons (XX) of 1 L WS2 (i.e., intralayer excitons) were observed in the heterostructure at 3 K at 594, 601, and 606 nm in the deconvoluted PL spectra, respectively. Notably, a broad and intense PL emission mainly due to HIXs in the heterostructure was observed in the visible-light region at 675–700 nm (below 200 K). All of the PL peaks corresponding to the characteristic excitons in the heterostructure were red-shifted with increasing temperature owing to the enhancement of electron–phonon interactions. Interestingly, with increasing excitation power, the PL peaks of HIXs in the heterostructure were significantly blue-shifted, while those corresponding to the X0 , X– , and XX of WS2 were red-shifted. These changes originate from the screening effect of the Coulomb and repulsive interactions between the dipole-aligned HIXs. Notably, the 4.22 ns lifetime of HIXs in the heterostructure obtained from the time-resolved PL decay curves at 3 K was significantly long and 8.6 times longer than that of the intralayer excitons. This study provides an understanding of HIXs in 2D heterostructures, which provide promising platforms for applications in nanoscale light-emitting diodes, sensors, and photovoltaics. [ABSTRACT FROM AUTHOR]- Published
- 2022
- Full Text
- View/download PDF
23. Optical response of WSe2-based vertical tunneling junction.
- Author
-
Walczyk, K., Krasucki, G., Olkowska-Pucko, K., Chen, Z., Taniguchi, T., Watanabe, K., Babiński, A., Koperski, M., Molas, M.R., and Zawadzka, N.
- Subjects
- *
CARRIER density , *PHOTOLUMINESCENCE , *LOW temperatures , *MONOMOLECULAR films , *VOLTAGE - Abstract
Layered materials have attracted significant interest because of their unique properties. Van der Waals heterostructures based on transition-metal dichalcogenides have been extensively studied because of potential optoelectronic applications. We investigate the optical response of a light-emitting tunneling structure based on a WSe 2 monolayer as an active emission material using the photoluminescence (PL) and electroluminescence (EL) experiments performed at low temperature of 5 K. We found that the application of the bias voltage allows us to change both a sign and a value of free carriers concentrations. Consequently, we address the several excitonic complexes emerging in PL spectra under applied bias voltage. The EL signal was also detected and ascribed to the emission in a high-carrier-concentration regime. The results show that the excitation mechanisms in the PL and EL are different, resulting in various emissions in both types of experimental techniques. • The optical response of a tunneling structure based on a WSe 2 monolayer was studied. • The emission lines apparent in the photoluminescence spectra were identified. • The electroluminescence in the high electrical bias regime was analyzed. [ABSTRACT FROM AUTHOR]
- Published
- 2025
- Full Text
- View/download PDF
24. Defect Formation of Light-Emitting Particles during the Synthesis of a Hierarchical Porous Surface of ZnO/SiO2/Si Structures
- Author
-
Rashid Zhapakov, Mykhail Begunov, Tatyana Seredavina, Danatbek Murzalinov, Abay Serikkanov, Elena Dmitriyeva, Sultan Zhantuarov, and Sayara Ibraimova
- Subjects
ZnO ,photoluminescence ,exciton ,oxygen vacancies ,porous silicon ,Engineering machinery, tools, and implements ,TA213-215 - Abstract
The formation of structures of different sizes on the surface of a single sample and the study of the mechanisms of their excitations and energy transitions is a promising area of research. ZnO/SiO2/Si heterostructures were formed by two-stage electrochemical etching of silicon wafers and synthesizing zinc oxide nanoparticles using sol-gel technology. By scanning electron and atomic force microscopies, various pores and clusters were identified. The presence of five levels of surface hierarchy provided the synthesis of light-emitting particles with different properties. Light emission mechanisms are associated with the recombination of excitons and the hyperfine structure of charged particles trapped on oxygen vacancy.
- Published
- 2023
- Full Text
- View/download PDF
25. Temperature-Dependent Exciton Dynamics in a Single GaAs Quantum Ring and a Quantum Dot.
- Author
-
Kim, Heedae, Kim, Jong Su, and Song, Jin Dong
- Subjects
- *
QUANTUM rings , *EXCITON theory , *EXCITON-phonon interactions , *AUDITING standards , *GALLIUM arsenide , *EXCITED states - Abstract
Micro-photoluminescence was observed while increasing the excitation power in a single GaAs quantum ring (QR) at 4 K. Fine structures at the energy levels of the ground (N = 1) and excited (N = 2) state excitons exhibited a blue shift when excitation power increased. The excited state exciton had a strong polarization dependence that stemmed from the asymmetric localized state. According to temperature-dependence measurements, strong exciton–phonon interaction (48 meV) was observed from an excited exciton state in comparison with the weak exciton–phonon interaction (27 meV) from the ground exciton state, resulting from enhanced confinement in the excited exciton state. In addition, higher activation energy (by 20 meV) was observed for the confined electrons in a single GaAs QR, where the confinement effect was enhanced by the asymmetric ring structure. [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF
26. Orientation-Mediated Luminescence Enhancement and Spin-Orbit Coupling in ZnO Single Crystals.
- Author
-
Hassan, Ali, Khan, Abbas Ahmad, Ahn, Yeong Hwan, Azam, Muhammad, Zubair, Muhammad, Xue, Wei, and Cao, Yu
- Subjects
- *
SPIN-orbit interactions , *SINGLE crystals , *LUMINESCENCE , *ZINC oxide , *LUMINESCENCE spectroscopy , *LOW temperatures , *OPTOELECTRONIC devices , *SUPERCONTINUUM generation - Abstract
Temperature-, excitation wavelength-, and excitation power-dependent photoluminescence (PL) spectroscopy have been utilized to investigate the orientation-modulated near band edge emission (NBE) and deep level emission (DLE) of ZnO single crystals (SCs). The near-band-edge emission of ZnO SC with <0001> orientation exhibits strong and sharp emission intensity with suppressed deep level defects (mostly caused by oxygen vacancies Vo). Furthermore, Raman analysis reveals that <0001> orientation has dominant E2 (high) and E2 (low) modes, indicating that this direction has better crystallinity. At low temperature, the neutral donor-to-bound exciton (DoX) transition dominates, regardless of the orientation, according to the temperature-dependent PL spectra. Moreover, free-exciton (FX) transition emerges at higher temperatures in all orientations. The PL intensity dependence on the excitation power has been described in terms of power-law (I~Lα). Our results demonstrate that the α for <0001>, <1120>, and <1010> is (1.148), (1.180), and (1.184) respectively. In short, the comprehensive PL analysis suggests that DoX transitions are dominant in the NBE region, whereas oxygen vacancies (Vo) are the dominant deep levels in ZnO. In addition, the <0001> orientation contains fewer Vo-related defects with intense excitonic emission in the near band edge region than other counterparts, even at high temperature (~543 K). These results indicate that <0001> growth direction is favorable for fabricating ZnO-based highly efficient optoelectronic devices. [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF
27. Photoluminescence side band spectroscopy of individual single-walled carbon nanotubes
- Author
-
Weisman, R. [Rice Univ., Houston, TX (United States)]
- Published
- 2016
- Full Text
- View/download PDF
28. Multiple Exciton Dynamics in MoS2 Nanosheet/Poly(methyl methacrylate)/Polyaniline Composites and Nonlinear Optical Properties: Implications for Saturable Absorber Applications.
- Author
-
Paul, Swati and Balasubramanian, Karthikeyan
- Abstract
Here, we demonstrate an efficient nanocomposite system for the enhancement of optical properties via a self-assembled 2D nanoarchitecture combined with insulating and conducting polymers. The excitonic properties of the ternary composites consisting of MoS
2 nanosheets, poly methyl methacrylate (PMMA), and polyaniline (PANI) (MPP) were tuned by optimizing the concentration of PANI. Their absorption spectra revealed a strong excitonic coupling between the components. The mechanisms of exciton dissociation and generation of interlayer excitons were investigated by steady-state and transient photoluminescence spectroscopy. The exciton decay time is reduced by almost 95% in the ternary composite at an optimized concentration of PANI than in pure MoS2 . This indicates a fast excitonic interaction between MoS2 and PANI in the presence of the insulating polymer PMMA. Furthermore, nonlinear optical studies using the z-scan technique further confirmed the exciton–exciton coupling in the ternary composites. Therefore, these ternary composites having multiple excitons and strong saturable absorption (SA) behavior provide a perspective for next-generation saturable absorber devices and other optoelectronic applications. [ABSTRACT FROM AUTHOR]- Published
- 2022
- Full Text
- View/download PDF
29. The Sign of Exciton-Photon Coupling in GaN-Based Triangular-like Ridge Cavity.
- Author
-
Zhou, Jing, Chen, Peng, Xie, Zili, Xiu, Xiangqian, Chen, Dunjun, Han, Ping, Shi, Yi, Zhang, Rong, and Zheng, Youdou
- Subjects
ANDERSON localization ,EXCITON theory ,PHOTOLUMINESCENCE measurement ,PHOTOLUMINESCENCE ,PHOTONS - Abstract
In this paper, the behavior of exciton radiative recombination in a GaN-based triangular-like ridge cavity is studied at room-temperature. The triangular-like ridge cavity is fabricated on a standard-blue-LED epitaxial wafer grown on a sapphire substrate. Through the photoluminescence (PL) and time-resolved photoluminescence (TR-PL) measurements, a clear modulation of the original spontaneous emission is found in the microcavity, a new transition channel is observed, and the effect is angle-dependent. Furthermore, by changing the tilt angle during angle-resolution photoluminescence (AR-PL), it is found that the coupling between excitons and photons in the cavity is the strongest when tilted at 10°. By simulation, the strong localization of photons in the top of the cavity can be confirmed. The PL, TR-PL, and AR-PL results showed the sign of the exciton-photon coupling in the triangular-like ridge cavity. [ABSTRACT FROM AUTHOR]
- Published
- 2022
- Full Text
- View/download PDF
30. All-optical dynamic tuning of local excitonic emission of monolayer MoS2 by integration with Ge2Sb2Te5
- Author
-
Ouyang Hao, Chen Haitao, Tang Yuxiang, Zhang Jun, Zhang Chenxi, Zhang Bin, Cheng Xiang’ai, and Jiang Tian
- Subjects
2d materials ,exciton ,all-optical ,integration ,photoluminescence ,Physics ,QC1-999 - Abstract
Strong quantum confinement and coulomb interactions induce tightly bound quasiparticles such as excitons and trions in an atomically thin layer of transitional metal dichalcogenides (TMDs), which play a dominant role in determining their intriguing optoelectronic properties. Thus, controlling the excitonic properties is essential for the applications of TMD-based devices. Here, we demonstrate the all-optical tuning of the local excitonic emission from a monolayer MoS2 hybridized with phase-change material Ge2Sb2Te5 (GST) thin film. By applying pulsed laser with different power on the MoS2/GST heterostructure, the peak energies of the excitonic emission of MoS2 can be tuned up to 40 meV, and the exciton/trion intensity ratio can be tuned by at least one order of magnitude. Raman spectra and transient pump-probe measurements show that the tunability originated from the laser-induced phase change of the GST thin film with charge transferring from GST to the monolayer MoS2. The dynamic tuning of the excitonic emission was all done with localized laser pulses and could be scaled readily, which pave a new way of controlling the excitonic emission in TMDs. Our findings could be potentially used as all-optical modulators or switches in future optical networks.
- Published
- 2020
- Full Text
- View/download PDF
31. Optical Properties of Conical Quantum Dot: Exciton-Related Raman Scattering, Interband Absorption and Photoluminescence
- Author
-
Sargis P. Gavalajyan, Grigor A. Mantashian, Gor Ts. Kharatyan, Hayk A. Sarkisyan, Paytsar A. Mantashyan, Sotirios Baskoutas, and David B. Hayrapetyan
- Subjects
conical quantum dot ,exciton ,Raman scattering ,interband absorption ,photoluminescence ,Chemistry ,QD1-999 - Abstract
The current work used the effective mass approximation conjoined with the finite element method to study the exciton states in a conical GaAs quantum dot. In particular, the dependence of the exciton energy on the geometrical parameters of a conical quantum dot has been studied. Once the one-particle eigenvalue equations have been solved, both for electrons and holes, the available information on energies and wave functions is used as input to calculate exciton energy and the effective band gap of the system. The lifetime of an exciton in a conical quantum dot has been estimated and shown to be in the range of nanoseconds. In addition, exciton-related Raman scattering, interband light absorption and photoluminescence in conical GaAs quantum dots have been calculated. It has been shown that with a decrease in the size of the quantum dot, the absorption peak has a blue shift, which is more pronounced for quantum dots of smaller sizes. Furthermore, the interband optical absorption and photoluminescence spectra have been revealed for different sizes of GaAs quantum dot.
- Published
- 2023
- Full Text
- View/download PDF
32. Br-substituent effect on photoluminescence and scintillation properties of (C6H5C2H4NH3)2PbCl4 perovskite-type compounds.
- Author
-
Matsuzawa, Shun, Okazaki, Kai, Nakauchi, Daisuke, Kawano, Naoki, Suto, Takeru, Kato, Takumi, Kawaguchi, Noriaki, and Yanagida, Takayuki
- Subjects
- *
PHOTOLUMINESCENCE , *DECAY constants , *SCINTILLATORS , *EXCITON theory , *LUMINESCENCE , *CRYSTALS - Abstract
The photoluminescence and scintillation properties of n-bromophenethylammonium lead chloride ((n-BrPEA) 2 PbCl 4) (n = 4, 3, and 2) and phenethylammonium lead chloride ((PEA) 2 PbCl 4) have been investigated. All the samples showed broad emission peaks at 400–700 nm upon excitation by UV light or X-ray. The decay time constants of 8–28 ns were obtained which originated from the recombination of self-trapped exciton (STE) within inorganic layers. The afterglow levels at 20 ms after 2 ms of X-ray irradiation of (4-BrPEA) 2 PbCl 4 and (3-BrPEA) 2 PbCl 4 (76 and 55 ppm) were better than (PEA) 2 PbCl 4 (379 ppm). The light yield of (4-BrPEA) 2 PbCl 4 (3100 photons/5.5 MeV-α) was higher than (PEA) 2 PbCl 4 (1400 photons/5.5 MeV-α). • (BrC 6 H 4 C 2 H 4 NH 3) 2 PbCl 4 crystals were grown by the slow cooling method. • All the crystals showed the luminescence due to the recombination of the self-trapped excitons confined in inorganic layers. • The (4-BrC 6 H 4 C 2 H 4 NH 3) 2 PbCl 4 crystal showed the highest QY in the present crystals. • The light yields of the (4-BrC 6 H 4 C 2 H 4 NH 3) 2 PbCl 4 crystals surpassed that of the unsubstituted crystal. [ABSTRACT FROM AUTHOR]
- Published
- 2024
- Full Text
- View/download PDF
33. Dot-Size Dependent Excitons in Droplet-Etched Cone-Shell GaAs Quantum Dots
- Author
-
Christian Heyn, Andreas Gräfenstein, Geoffrey Pirard, Leonardo Ranasinghe, Kristian Deneke, Ahmed Alshaikh, Gabriel Bester, and Wolfgang Hansen
- Subjects
quantum dot ,droplet etching ,photoluminescence ,exciton ,biexciton ,lifetime ,Chemistry ,QD1-999 - Abstract
Strain-free GaAs quantum dots (QDs) are fabricated by filling droplet-etched nanoholes in AlGaAs. Using a template of nominally identical nanoholes, the QD size is precisely controlled by the thickness of the GaAs filling layer. Atomic force microscopy indicates that the QDs have a cone-shell shape. From single-dot photoluminescence measurements, values of the exciton emission energy (1.58...1.82 eV), the exciton–biexciton splitting (1.8...2.5 meV), the exciton radiative lifetime of bright (0.37...0.58 ns) and dark (3.2...6.7 ns) states, the quantum efficiency (0.89...0.92), and the oscillator strength (11.2...17.1) are determined as a function of the dot size. The experimental data are interpreted by comparison with an atomistic model.
- Published
- 2022
- Full Text
- View/download PDF
34. Electronic Band Transitions in γ-Ge3N4.
- Author
-
Feldbach, Eduard, Zerr, Andreas, Museur, Luc, Kitaura, Mamoru, Manthilake, Geeth, Tessier, Franck, Krasnenko, Veera, and Kanaev, Andrei
- Abstract
Electronic band structure in germanium nitride having spinel structure, γ-Ge
3 N4 , was examined using two spectroscopic techniques, cathodoluminescence and synchrotron-based photoluminescence. The sample purity was confirmed by x-ray diffraction and Raman analyses. The spectroscopic measurements provided first experimental evidence of a large free exciton binding energy De ≈0.30 eV and direct interband transitions in this material. The band gap energy Eg = 3.65 ± 0.05 eV measured with a higher precision was in agreement with that previously obtained via XES/XANES method. The screened hybrid functional Heyd–Scuseria–Ernzerhof (HSE06) calculations of the electronic structure supported the experimental results. Based on the experimental data and theoretical calculations, the limiting efficiency of the excitation conversion to light was estimated and compared with that of w-GaN, which is the basic material of commercial light emitting diodes. The high conversion efficiency, very high hardness and rigidity combined with a thermal stability in air up to ~ 700 °C reveal the potential of γ-Ge3 N4 for robust and efficient photonic emitters. [ABSTRACT FROM AUTHOR]- Published
- 2021
- Full Text
- View/download PDF
35. Ultrafast carrier dynamics in organic-inorganic semiconductor nanostructures
- Author
-
Yong, Chaw Keong and Herz, Laura
- Subjects
620.5 ,Advanced materials ,Nanomaterials ,Microscopy ,Laser Spectroscopy ,Photochemistry and reaction dynamics ,Spectroscopy and molecular structure ,Nanostructures ,Materials processing ,Semiconductor devices ,Processing of advanced materials ,Single crystal semiconductors ,Condensed Matter Physics ,ultrafast spectroscopy ,photoluminescence ,Mott transition ,semiconductor nanowires ,exciton ,carrier cooling ,hot-carrier ,type-II heterojunctions ,charge transfer ,carrier dynamics ,lifetime ,doping ,trapping - Abstract
This thesis is concerned with the influence of nanoscale boundaries and interfaces upon the electronic processes that occur within the inorganic semiconductors. Inorganic semiconductor nanowires and their blends with semiconducting polymers have been investigated using state-of-the-art ultrafast optical techniques to provide information on the sub-picosecond to nanosecond photoexcitation dynamics in these systems. Chapters 1 and 2 introduce the theory and background behind the work and present a literature review of previous work utilising nanowires in hybrid organic photovoltaic devices, revealing the performances to date. The experimental methods used during the thesis are detailed in Chapter 3. Chapter 4 describes the crucial roles of surface passivation on the ultrafast dynamics of exciton formation in gallium arsenide (GaAs) nanowires. By passivating the surface states of nanowires, exciton formation via the bimolecular conversion of electron-hole plasma can observed over few hundred picoseconds, in-contrast to the fast carrier trapping in 10 ps observed in the uncoated nanowires. Chapter 5 presents a novel method to passivate the surface-states of GaAs nanowires using semiconducting polymer. The carrier lifetime in the nanowires can be strongly enhanced when the ionization potential of the overcoated semiconducting polymer is smaller than the work function of the nanowires and the surface native oxide layers of nanowires are removed. Finally, Chapter 6 shows that the carrier cooling in the type-II wurtzite-zincblend InP nanowires is reduced by order-of magnitude during the spatial charge-transfer across the type-II heterojunction. The works decribed in this thesis reveals the crucial role of surface-states and bulk defects on the carrier dynamics of semiconductor nanowires. In-addition, a novel approach to passivate the surface defect states of nanowires using semiconducting polymers was developed.
- Published
- 2012
36. Temperature-Dependent Exciton Dynamics in a Single GaAs Quantum Ring and a Quantum Dot
- Author
-
Heedae Kim, Jong Su Kim, and Jin Dong Song
- Subjects
quantum ring structure ,quantum dot structure ,exciton ,photoluminescence ,localized states ,polarization dependence ,Chemistry ,QD1-999 - Abstract
Micro-photoluminescence was observed while increasing the excitation power in a single GaAs quantum ring (QR) at 4 K. Fine structures at the energy levels of the ground (N = 1) and excited (N = 2) state excitons exhibited a blue shift when excitation power increased. The excited state exciton had a strong polarization dependence that stemmed from the asymmetric localized state. According to temperature-dependence measurements, strong exciton–phonon interaction (48 meV) was observed from an excited exciton state in comparison with the weak exciton–phonon interaction (27 meV) from the ground exciton state, resulting from enhanced confinement in the excited exciton state. In addition, higher activation energy (by 20 meV) was observed for the confined electrons in a single GaAs QR, where the confinement effect was enhanced by the asymmetric ring structure.
- Published
- 2022
- Full Text
- View/download PDF
37. Orientation-Mediated Luminescence Enhancement and Spin-Orbit Coupling in ZnO Single Crystals
- Author
-
Ali Hassan, Abbas Ahmad Khan, Yeong Hwan Ahn, Muhammad Azam, Muhammad Zubair, Wei Xue, and Yu Cao
- Subjects
zinc oxide ,single crystal ,photoluminescence ,exciton ,impurities and defects ,Chemistry ,QD1-999 - Abstract
Temperature-, excitation wavelength-, and excitation power-dependent photoluminescence (PL) spectroscopy have been utilized to investigate the orientation-modulated near band edge emission (NBE) and deep level emission (DLE) of ZnO single crystals (SCs). The near-band-edge emission of ZnO SC with orientation exhibits strong and sharp emission intensity with suppressed deep level defects (mostly caused by oxygen vacancies Vo). Furthermore, Raman analysis reveals that orientation has dominant E2 (high) and E2 (low) modes, indicating that this direction has better crystallinity. At low temperature, the neutral donor-to-bound exciton (DoX) transition dominates, regardless of the orientation, according to the temperature-dependent PL spectra. Moreover, free-exciton (FX) transition emerges at higher temperatures in all orientations. The PL intensity dependence on the excitation power has been described in terms of power-law (I~Lα). Our results demonstrate that the α for , , and is (1.148), (1.180), and (1.184) respectively. In short, the comprehensive PL analysis suggests that DoX transitions are dominant in the NBE region, whereas oxygen vacancies (Vo) are the dominant deep levels in ZnO. In addition, the orientation contains fewer Vo-related defects with intense excitonic emission in the near band edge region than other counterparts, even at high temperature (~543 K). These results indicate that growth direction is favorable for fabricating ZnO-based highly efficient optoelectronic devices.
- Published
- 2022
- Full Text
- View/download PDF
38. Giant enhancement of photoluminescence emission in monolayer WS2 by femtosecond laser irradiation.
- Author
-
Qin, Cheng-Bing, Liang, Xi-Long, Han, Shuang-Ping, Zhang, Guo-Feng, Chen, Rui-Yun, Hu, Jian-Yong, Xiao, Lian-Tuan, and Jia, Suo-Tang
- Abstract
Monolayer transition metal dichalcogenides have emerged as promising materials for optoelectronic and nanophotonic devices. However, the low photoluminescence (PL) quantum yield (QY) hinders their various potential applications. Here we engineer and enhance the PL intensity of monolayer WS
2 by femtosecond laser irradiation. More than two orders of magnitude enhancement of PL intensity as compared to the as-prepared sample is determined. Furthermore, the engineering time is shortened by three orders of magnitude as compared to the improvement of PL intensity by continuous-wave laser irradiation. Based on the evolution of PL spectra, we attribute the giant PL enhancement to the conversion from trion emission to exciton, as well as the improvement of the QY when exciton and trion are localized to the new-formed defects. We have created microstructures on the monolayer WS2 based on the enhancement of PL intensity, where the engineered structures can be stably stored for more than three years. This flexible approach with the feature of excellent long-term storage stability is promising for applications in information storage, display technology, and optoelectronic devices. [ABSTRACT FROM AUTHOR]- Published
- 2021
- Full Text
- View/download PDF
39. All-optical dynamic tuning of local excitonic emission of monolayer MoS2 by integration with Ge2Sb2Te5.
- Author
-
Ouyang, Hao, Chen, Haitao, Tang, Yuxiang, Zhang, Jun, Zhang, Chenxi, Zhang, Bin, Cheng, Xiang'ai, and Jiang, Tian
- Subjects
MONOMOLECULAR films ,PULSED lasers ,PHASE change materials ,LASER pulses ,THIN films - Abstract
Strong quantum confinement and coulomb interactions induce tightly bound quasiparticles such as excitons and trions in an atomically thin layer of transitional metal dichalcogenides (TMDs), which play a dominant role in determining their intriguing optoelectronic properties. Thus, controlling the excitonic properties is essential for the applications of TMD-based devices. Here, we demonstrate the all-optical tuning of the local excitonic emission from a monolayer MoS
2 hybridized with phase-change material Ge2 Sb2 Te5 (GST) thin film. By applying pulsed laser with different power on the MoS2 /GST heterostructure, the peak energies of the excitonic emission of MoS2 can be tuned up to 40 meV, and the exciton/trion intensity ratio can be tuned by at least one order of magnitude. Raman spectra and transient pump-probe measurements show that the tunability originated from the laser-induced phase change of the GST thin film with charge transferring from GST to the monolayer MoS2 . The dynamic tuning of the excitonic emission was all done with localized laser pulses and could be scaled readily, which pave a new way of controlling the excitonic emission in TMDs. Our findings could be potentially used as all-optical modulators or switches in future optical networks. [ABSTRACT FROM AUTHOR]- Published
- 2020
- Full Text
- View/download PDF
40. SYNTHESIS AND PHOTOLUMINESCENCE STUDIES ON ZINC OXIDE NANOWIRES
- Author
-
Nguyen Ngoc Long, Ngo Xuan Dai, and Nguyen Thi Thuc Hien
- Subjects
Semiconductors ,nanostructures ,photoluminescence ,exciton ,zinc oxide ,Technology (General) ,T1-995 ,Science (General) ,Q1-390 - Abstract
Semiconductor single crystal ZnO nanowires have been successfully synthesized by a simple method based on thermal evaporation of ZnO powders mixed with graphite. Metallic catalysts, carrying gases, and vacuum conditions are not necessary. The x-ray diffraction (XRD) analysis shows that the ZnO nanowires are highly crystallized and have a typical wurtzite hexagonal structure with lattice constants a = 0.3246 nm and c = 0.5203 nm. The scanning electron microscopy (SEM) images of nanowires indicate that diameters of the ZnO nanowires normally range from 100 to 300 nm and their lengths are several tens of micrometers. Photoluminescence (PL) and photoluminescence excitation (PLE) spectra of the nanowires were measured in the range of temperature from 15 K to the room temperature. Photoluminescence spectra at low temperatures exhibit a group of ultraviolet (UV) narrow peaks in the region 368 nm ~ 390 nm, and a blue-green very broad peak at 500 nm. Origin of the emission lines in PL spectra and the lines in PLE spectra is discussed.
- Published
- 2017
- Full Text
- View/download PDF
41. Photoluminescence Investigation of the InP/ZnS Quantum Dots and Their Coupling with the Au Nanorods.
- Author
-
Chen, Tingting, Li, Ke, Mao, Huibing, Chen, Ye, Wang, Jiqing, and Weng, Guoen
- Subjects
PHOTOLUMINESCENCE ,QUANTUM dots ,SILVER ,NANORODS ,SURFACE plasmon resonance - Abstract
The photoluminescence spectra of the InP/ZnS quantum dots (QDs) and the composite structure of the InP/ZnS QDs coupled with Au nanorods are investigated in this paper. In the luminescence spectra of the two samples, the recombination of the bright–dark doublet exciton states and an upper bright exciton state are observed at the temperature 11–130 K. The temperature dependence of the main emission peaks of the InP/ZnS QDs and the composite structure can be expressed by the Varshni expression in the temperature range of 11–300 K. The coupling between the QDs and the surface plasmon resonance (SPR) states has a great effect on the exciton recombination and the defect recombination. Because of the coupling, the variation range of the main emission peak of the composite structure is about 28 meV more than the pure QDs with the temperature from 11 K to 300 K. The red shift of the defect emission with increasing temperature is coincident with the red shift of the SPR energy with increasing temperature. The experimental results confirm that the energy transfer from the SPR states is the main source of the defect emission. [ABSTRACT FROM AUTHOR]
- Published
- 2019
- Full Text
- View/download PDF
42. Observation of chiral surface excitons in a topological insulator Bi2Se3.
- Author
-
Kung, H.-H., Goyal, A. P., Maslov, D. L., Wang, X., Lee, A., Kemper, A. F., Cheong, S.-W., and Blumberg, G.
- Subjects
- *
TOPOLOGICAL insulators , *EXCITON theory , *PHOTOLUMINESCENCE , *ELECTRONS , *COULOMB functions - Abstract
The protected electron states at the boundaries or on the surfaces of topological insulators (TIs) have been the subject of intense theoretical and experimental investigations. Such states are enforced by very strong spin-orbit interaction in solids composed of heavy elements. Here, we study the composite particles--chiral excitons--formed by the Coulomb attraction between electrons and holes residing on the surface of an archetypical 3D TI, Bi2Se3. Photoluminescence (PL) emission arising due to recombination of excitons in conventional semiconductors is usually unpolarized because of scattering by phonons and other degrees of freedom during exciton thermalization. On the contrary, we observe almost perfectly polarization-preserving PL emission from chiral excitons. We demonstrate that the chiral excitons can be optically oriented with circularly polarized light in a broad range of excitation energies, even when the latter deviate fromthe (apparent) optical band gap by hundreds of millielectronvolts, and that the orientation remains preserved even at room temperature. Based on the dependences of the PL spectra on the energy and polarization of incident photons, we propose that chiral excitons are made from massive holes and massless (Dirac) electrons, both with chiral spin textures enforced by strong spin-orbit coupling. A theoretical model based on this proposal describes quantitatively the experimental observations. The optical orientation of composite particles, the chiral excitons, emerges as a general result of strong spin-orbit coupling in a 2D electron system. Our findings can potentially expand applications of TIs in photonics and optoelectronics. [ABSTRACT FROM AUTHOR]
- Published
- 2019
- Full Text
- View/download PDF
43. Observation of chiral surface excitons in a topological insulator Bi2Se3.
- Author
-
Kung, H.-H., Goyal, A. P., Maslov, D. L., Wang, X., Lee, A., Kemper, A. F., Cheong, S.-W., and Blumberg, G.
- Subjects
TOPOLOGICAL insulators ,EXCITON theory ,PHOTOLUMINESCENCE ,ELECTRONS ,COULOMB functions - Abstract
The protected electron states at the boundaries or on the surfaces of topological insulators (TIs) have been the subject of intense theoretical and experimental investigations. Such states are enforced by very strong spin-orbit interaction in solids composed of heavy elements. Here, we study the composite particles--chiral excitons--formed by the Coulomb attraction between electrons and holes residing on the surface of an archetypical 3D TI, Bi2Se3. Photoluminescence (PL) emission arising due to recombination of excitons in conventional semiconductors is usually unpolarized because of scattering by phonons and other degrees of freedom during exciton thermalization. On the contrary, we observe almost perfectly polarization-preserving PL emission from chiral excitons. We demonstrate that the chiral excitons can be optically oriented with circularly polarized light in a broad range of excitation energies, even when the latter deviate fromthe (apparent) optical band gap by hundreds of millielectronvolts, and that the orientation remains preserved even at room temperature. Based on the dependences of the PL spectra on the energy and polarization of incident photons, we propose that chiral excitons are made from massive holes and massless (Dirac) electrons, both with chiral spin textures enforced by strong spin-orbit coupling. A theoretical model based on this proposal describes quantitatively the experimental observations. The optical orientation of composite particles, the chiral excitons, emerges as a general result of strong spin-orbit coupling in a 2D electron system. Our findings can potentially expand applications of TIs in photonics and optoelectronics. [ABSTRACT FROM AUTHOR]
- Published
- 2019
- Full Text
- View/download PDF
44. PLQ−sim: A computational tool for simulating photoluminescence quenching dynamics in organic donor/acceptor blends.
- Author
-
Benatto, Leandro, Mesquita, Omar, Roman, Lucimara S., Capaz, Rodrigo B., Candiotto, Graziâni, and Koehler, Marlus
- Subjects
- *
ELECTRON donors , *PHOTOLUMINESCENCE , *ORGANIC semiconductors , *CHARGE transfer , *ENERGY transfer , *FREEWARE (Computer software) - Abstract
Photoluminescence Quenching Simulator (PLQ−Sim) is a user−friendly software to study the photoexcited state dynamics at the interface between two organic semiconductors forming a blend: an electron donor (D), and an electron acceptor (A). Its main function is to provide substantial information on the photophysical processes relevant to organic photovoltaic and photothermal devices, such as charge transfer state formation and subsequent free charge generation or exciton recombination. From input parameters provided by the user, the program calculates the transfer rates of the D/A blend and employs a kinetic model that provides the photoluminescence quenching efficiency for initial excitation in the donor or acceptor. When calculating the rates, the user can choose to use disorder parameters to better describe the system. In addition, the program was developed to address energy transfer phenomena that are commonly present in organic blends. The time evolution of state populations is also calculated providing relevant information for the user. In this article, we present the theory behind the kinetic model, along with suggestions for methods to obtain the input parameters. A detailed demonstration of the program, its applicability, and an analysis of the outputs are also presented. PLQ−Sim is license free software that can be run via dedicated webserver nanocalc.org or downloading the program executables (for Unix , Windows , and macOS) from the PLQ-Sim repository on GitHub. [ABSTRACT FROM AUTHOR]
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- 2024
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45. Single- and narrow-line photoluminescence in a boron nitride-supported MoSe 2 /graphene heterostructure
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Loïc Moczko, Aditya Singh, Michelangelo Romeo, Etienne Lorchat, Joanna Wolff, Kenji Watanabe, Luis E. Parra López, Stéphane Berciaud, and Takashi Taniguchi
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Materials science ,Photoluminescence ,Exciton ,FOS: Physical sciences ,General Physics and Astronomy ,01 natural sciences ,7. Clean energy ,010305 fluids & plasmas ,law.invention ,Condensed Matter::Materials Science ,chemistry.chemical_compound ,law ,Mesoscale and Nanoscale Physics (cond-mat.mes-hall) ,0103 physical sciences ,Monolayer ,010306 general physics ,Condensed Matter - Materials Science ,Condensed Matter - Mesoscale and Nanoscale Physics ,business.industry ,Graphene ,Doping ,Materials Science (cond-mat.mtrl-sci) ,Heterojunction ,Condensed Matter::Mesoscopic Systems and Quantum Hall Effect ,3. Good health ,chemistry ,Boron nitride ,Optoelectronics ,business ,Bilayer graphene - Abstract
Heterostructures made from van der Waals materials provide a template to investigate proximity effects at atomically sharp heterointerfaces. In particular, near-field charge and energy transfer in heterostructures made from semiconducting transition metal dichalcogenides (TMD) have attracted interest to design model 2D "donor-acceptor" systems and new optoelectronic components. Here, using of Raman scattering and photoluminescence spectroscopies, we report a comprehensive characterization of a molybedenum diselenide (MoSe$_2$) monolayer deposited onto hexagonal boron nitride (hBN) and capped by mono- and bilayer graphene. Along with the atomically flat hBN susbstrate, a single graphene epilayer is sufficient to passivate the MoSe$_2$ layer and provides a homogenous environment without the need for an extra capping layer. As a result, we do not observe photo-induced doping in our heterostructure and the MoSe$_2$ excitonic linewidth gets as narrow as 1.6~meV, hence approaching the homogeneous limit. The semi-metallic graphene layer neutralizes the 2D semiconductor and enables picosecond non-radiative energy transfer that quenches radiative recombination from long-lived states. Hence, emission from the neutral band edge exciton largely dominates the photoluminescence spectrum of the MoSe$_2$/graphene heterostructure. Since this exciton has a picosecond radiative lifetime at low temperature, comparable with the energy transfer time, its low-temperature photoluminescence is only quenched by a factor of $3.3 \pm 1$ and $4.4 \pm 1$ in the presence of mono- and bilayer graphene, respectively. Finally, while our bare MoSe$_2$ on hBN exhibits negligible valley polarization at low temperature and under near-resonant excitation, we show that interfacing MoSe$_2$ with graphene yields a single-line emitter with degrees of valley polarization and coherence up to $\sim 15\,\%$., version 3, 5 figures
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- 2022
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46. Lower limits for non-radiative recombination loss in organic donor/acceptor complexes
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Yun Liu, Veaceslav Coropceanu, Zilong Zheng, David S. Ginger, and Jean-Luc Brédas
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Materials science ,Photoluminescence ,Organic solar cell ,Process Chemistry and Technology ,Exciton ,Acceptor ,Mechanics of Materials ,Chemical physics ,OLED ,Radiative transfer ,General Materials Science ,Quantum efficiency ,Electrical and Electronic Engineering ,Non-radiative recombination - Abstract
Understanding the factors controlling radiative and non-radiative transition rates for charge transfer states in organic systems is important for applications ranging from organic photovoltaics (OPV) to lasers and LEDs. We explore the role of charge-transfer (CT) energetics, lifetimes, and photovoltaic properties in the limit of very slow non-radiative rates by using a model donor/acceptor system with photoluminescence dominated by thermally activated delayed fluorescence (TADF). This blend exhibits an extremely high photoluminescence quantum efficiency (PLQY = ∼22%) and comparatively long PL lifetime, while simultaneously yielding appreciable amounts of free charge generation (photocurrent external quantum efficiency EQE of 24%). In solar cells, this blend exhibits non-radiative voltage losses of only ∼0.1 V, among the lowest reported for an organic system. Notably, we find that the non-radiative decay rate, knr, is on the order of 105 s−1, approximately 4–5 orders of magnitude slower than typical OPV blends, thereby confirming that high radiative efficiency and low non-radiative voltage losses are achievable by reducing knr. Furthermore, despite the high radiative efficiency and already comparatively slow knr, we find that knr is nevertheless much faster than predicted by Marcus–Levich–Jortner two-state theory and we conclude that CT-local exciton (LE) hybridization is present. Our findings highlight that it is crucial to evaluate how radiative and non-radiative rates of the LE states individually influence the PLQY of charge-transfer states, rather than solely focusing on the PLQY of the LE. This conclusion will guide material selection in achieving low non-radiative voltage loss in organic solar cells and high luminescence efficiency in organic LEDs.
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- 2022
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47. Exciton funneling amplified photoluminescence anisotropy in organic radical-doped microcrystals
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Yong Sheng Zhao, Chan Qiao, Yongli Yan, Zhonghao Zhou, and Jiannian Yao
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Photoluminescence ,Materials science ,Condensed Matter::Other ,business.industry ,Exciton ,Doping ,Physics::Optics ,General Chemistry ,Condensed Matter::Mesoscopic Systems and Quantum Hall Effect ,Condensed Matter::Materials Science ,Physics::Atomic and Molecular Clusters ,Materials Chemistry ,Optoelectronics ,Anisotropy ,Luminescence ,business - Abstract
We demonstrate a controllable photoluminescence anisotropy amplification in organic luminescent radical-doped microcrystals via exciton funneling. The widely tunable doping ratio resulting from very similar molecular structures between hosts and guests leads to a freely tailorable exciton funneling process, which paves an avenue for the construction of high-performance polarizing optical elements.
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- 2022
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48. Te4+-doped zero-dimensional Cs2ZnCl4 single crystals for broadband yellow light emission
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Yuexiao Pan, Xiaoxia Liu, Chengdong Peng, Daying Guo, and Lijie Zhang
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Materials science ,Photoluminescence ,business.industry ,Exciton ,Doping ,Phosphor ,General Chemistry ,Ion ,symbols.namesake ,Stokes shift ,Excited state ,Materials Chemistry ,symbols ,Optoelectronics ,Light emission ,business - Abstract
As an all-inorganic 0D lead-free metal halide, Cs2ZnCl4 is a potential excellent matrix to prepare chemical stable and environmentally friendly photoluminescent materials through ion doping strategy. So, it is necessary to study the emission property of every kind of doping ion in the tetrahedral coordination of Cs2ZnCl4 actually. Here, for the first time, we successfully synthesize the Te4+-doped Cs2ZnCl4 single crystals via a facile hydrothermal method. X-ray crystallography clearly reveals the strong distortion of the tetrahedral units in Cs2ZnCl4 caused by the doping of Te4+. Broadband yellow-light emission covering from 450 nm to 700 nm with a large Stokes shift is observed in Cs2ZnCl4:Te4+ single crystals and attributed to the self-trapped excitons (STEs) caused by the lattice vibration of the distorted structure. It is worth mentioning that this broadband yellow phosphor can be excited by a wide range of blue light, implicitly giving it excellent talent to adapt to multiple models of blue LED chips, thus serving as suitable yellow phosphor that can be applied to fabricate WLEDs without need to worry about the lack of red light.
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- 2022
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49. Short and long-range electron transfer compete to determine free-charge yield in organic semiconductors
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Seth R. Marder, Taylor G. Allen, Stephen Barlow, Bryon W. Larson, Garry Rumbles, Raghunath R. Dasari, Iryna Davydenko, Obadiah G. Reid, and Joshua M. Carr
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Materials science ,Photoluminescence ,Process Chemistry and Technology ,Exciton ,Electron donor ,Rate equation ,Photoinduced electron transfer ,Organic semiconductor ,Electron transfer ,Delocalized electron ,chemistry.chemical_compound ,chemistry ,Mechanics of Materials ,Chemical physics ,General Materials Science ,Electrical and Electronic Engineering - Abstract
Understanding how Frenkel excitons efficiently split to form free-charges in low-dielectric constant organic semiconductors has proven challenging, with many different models proposed in recent years to explain this phenomenon. Here, we present evidence that a simple model invoking a modest amount of charge delocalization, a sum over the available microstates, and the Marcus rate constant for electron transfer can explain many seemingly contradictory phenomena reported in the literature. We use an electron-accepting fullerene host matrix dilutely sensitized with a series of electron donor molecules to test this hypothesis. The donor series enables us to tune the driving force for photoinduced electron transfer over a range of 0.7 eV, mapping out normal, optimal, and inverted regimes for free-charge generation efficiency, as measured by time-resolved microwave conductivity. However, the photoluminescence of the donor is rapidly quenched as the driving force increases, with no evidence for inverted behavior, nor the linear relationship between photoluminescence quenching and charge-generation efficiency one would expect in the absence of additional competing loss pathways. This behavior is self-consistently explained by competitive formation of bound charge-transfer states and long-range or delocalized free-charge states, where both rate constants are described by the Marcus rate equation. Moreover, the model predicts a suppression of the inverted regime for high-concentration blends and efficient ultrafast free-charge generation, providing a mechanistic explanation for why Marcus-inverted-behavior is rarely observed in device studies.
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- 2022
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50. Photoluminescence-Linewidth-Derived Exciton Masses for InGaAsN Alloys
- Author
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MODINE, NORMAND
- Published
- 2001
- Full Text
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